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飞秒可调谐泵浦瞬态吸收测量揭示了高掺锗和低掺锗硅玻璃中点缺陷的光循环。

Photocycle of point defects in highly- and weakly-germanium doped silica revealed by transient absorption measurements with femtosecond tunable pump.

机构信息

UJM, CNRS, IOGS, Laboratoire H. Curien, UMRCNRS 5516, Univ Lyon, 42000, Saint-Étienne, France.

Department of Physics and Chemistry "Emilio Segrè", University of Palermo, Via Archirafi 36, 90123, Palermo, Italy.

出版信息

Sci Rep. 2022 Jun 2;12(1):9223. doi: 10.1038/s41598-022-13156-7.

DOI:10.1038/s41598-022-13156-7
PMID:35654982
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9163034/
Abstract

We report pump-probe transient absorption measurements addressing the photocycle of the Germanium lone pair center (GLPC) point defect with an unprecedented time resolution. The GLPC is a model point defect with a simple and well-understood electronic structure, highly relevant for several applications. Therefore, a full explanation of its photocycle is fundamental to understand the relaxation mechanisms of such molecular-like systems in solid state. The experiment, carried out exciting the sample resonantly with the ultraviolet (UV) GLPC absorption band peaked at 5.1 eV, gave us the possibility to follow the defect excitation-relaxation dynamics from the femto-picosecond to the nanosecond timescale in the UV-visible range. Moreover, the transient absorption signal was studied as a function of the excitation photon energy and comparative experiments were conducted on highly- and weakly-germanium doped silica glasses. The results offer a comprehensive picture of the relaxation dynamics of GLPC and allow observing the interplay between electronic transitions localized on the defect and those related to bandgap transitions, providing a clear evidence that the role of dopant high concentration is not negligible in the earliest dynamics.

摘要

我们报告了泵浦探针瞬态吸收测量结果，这些结果涉及到锗孤对中心（GLPC）点缺陷的光循环，其时间分辨率前所未有。GLPC 是一个具有简单而明确的电子结构的模型点缺陷，与几个应用高度相关。因此，对其光循环的充分解释对于理解固体状态中此类分子样系统的弛豫机制至关重要。实验中，我们通过与 5.1 eV 处紫外 GLPC 吸收带共振激发样品，使我们能够在飞秒到纳秒的时间尺度上在紫外可见范围内跟踪缺陷的激发-弛豫动力学。此外，我们还研究了瞬态吸收信号作为激发光子能量的函数，同时对高浓度和低浓度锗掺杂二氧化硅玻璃进行了对比实验。结果提供了 GLPC 弛豫动力学的综合图景，并允许观察局域在缺陷上的电子跃迁与带隙跃迁之间的相互作用，清楚地表明掺杂剂高浓度在最早的动力学中并非微不足道。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/ce0fcee9ca23/41598_2022_13156_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/b0513ba3d07a/41598_2022_13156_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/8c391bab0bb8/41598_2022_13156_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/267ffba6208b/41598_2022_13156_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/d062d5a05328/41598_2022_13156_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/362b401c2364/41598_2022_13156_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/ce0fcee9ca23/41598_2022_13156_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/b0513ba3d07a/41598_2022_13156_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/8c391bab0bb8/41598_2022_13156_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/267ffba6208b/41598_2022_13156_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/d062d5a05328/41598_2022_13156_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/362b401c2364/41598_2022_13156_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5313/9163034/ce0fcee9ca23/41598_2022_13156_Fig6_HTML.jpg

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本文引用的文献

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Transient absorption with a femtosecond tunable excitation pump reveals the emission kinetics of color centers in amorphous silica.利用飞秒可调谐激发泵浦进行的瞬态吸收揭示了非晶硅中色心的发射动力学。
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Radiation tolerant fiber Bragg gratings for high temperature monitoring at MGy dose levels.用于在兆戈瑞剂量水平下进行高温监测的耐辐射光纤布拉格光栅
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飞秒荧光研究紫外染料的振动弛豫和冷却动力学。
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